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Free keywords:
Silica; Ruthenium; Immobilized catalysts; Deuteron NMR
ruthenium
Abstract:
2H solid-state NMR measurements were performed on three samples of ruthenium nanoparticles synthesized inside two different kinds of mesoporous silica, namely SBA-3 silica materials and SBA-15 functionalized with –COOH groups and loaded with deuterium gas. The line-shape analyses of the spectra reveal the different deuteron species. In all samples a strong –OD signal is found, which shows the catalytic activity of the metal, which activates the D–D bond and deuterates the –SiOH groups through the gas phase, corroborating their usability as catalysts for hydrogenation reactions. At room temperature the mobility of the –Si–OD groups depends on the sample preparation. In addition to the –Si–OD deuterons, the presence of different types of deuterons bound to the metal is revealed. The singly coordinated –Ru–D species exhibit several different quadrupolar couplings, which indicate the presence of several non-equivalent binding sites with differing binding strength. In addition to the dissociated hydrogen species there is also a dihydrogen species –Ru–D2, which is attributed to defect sites on the surface. It exhibits a fast rotational dynamics at all temperatures. Finally there are also indications of three-fold coordinated surface deuterons and octahedrally coordinated deuterons inside the metal.
